Photoinduced phase nucleation driven by multiscale charge transfer and symmetry change dynamics

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Abstract Understanding photoinduced phase transitions is key for developing optoelectronic devices based on the ultrafast control of multifunctional materials. Still, how macroscopic transformations emerge from local excitations remains poorly understood, as it is experimentally challenging to isolate the multiscale electronic and structural dynamics. Here, we use femtosecond X-ray techniques to track the non-equilibrium dynamics leading to macroscopic transformation in a Prussian Blue analogue. The experimental data evidence a sequence of phenomena with different equilibration time scales. The initial electronic excitation leads to reverse Jahn-Teller distortion within 50 femtoseconds, which generates intermetallic charge-transfer polarons within 200 femtoseconds. Our study reveals how these photoinduced polarons generate significant lattice strain and trigger the phase nucleation within 60 picoseconds, where the lattice expansion leads to a self-amplifying macroscopic phase transition.
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Photoinduced phase nucleation driven by multiscale charge transfer and symmetry change dynamics | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Article Photoinduced phase nucleation driven by multiscale charge transfer and symmetry change dynamics Eric Collet, Marius Hervé, Gael Privault, Serhane Zerdane, Shintaro Agaki, and 6 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-6871744/v1 This work is licensed under a CC BY 4.0 License Status: Published Journal Publication published 19 Mar, 2026 Read the published version in Nature Materials → Version 1 posted You are reading this latest preprint version Abstract Understanding photoinduced phase transitions is key for developing optoelectronic devices based on the ultrafast control of multifunctional materials. Still, how macroscopic transformations emerge from local excitations remains poorly understood, as it is experimentally challenging to isolate the multiscale electronic and structural dynamics. Here, we use femtosecond X-ray techniques to track the non-equilibrium dynamics leading to macroscopic transformation in a Prussian Blue analogue. The experimental data evidence a sequence of phenomena with different equilibration time scales. The initial electronic excitation leads to reverse Jahn-Teller distortion within 50 femtoseconds, which generates intermetallic charge-transfer polarons within 200 femtoseconds. Our study reveals how these photoinduced polarons generate significant lattice strain and trigger the phase nucleation within 60 picoseconds, where the lattice expansion leads to a self-amplifying macroscopic phase transition. Physical sciences/Materials science/Condensed-matter physics/Phase transitions and critical phenomena Physical sciences/Materials science/Materials for optics/Ultrafast photonics Full Text Additional Declarations There is NO Competing Interest. Supplementary Files SupplementaryInformation.pdf Suppplementary Information SupplementaryVideoS1.mp4 Temporal evolution of the (111) Bragg peak SupplementaryVideoS2.mp4 Temporal evolution of the (200)/(002) Bragg peaks Methods.pdf Methods Cite Share Download PDF Status: Published Journal Publication published 19 Mar, 2026 Read the published version in Nature Materials → Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. 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